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1. In Situ Formation of Polymer-Inorganic Solid-Electrolyte Interphase for Stable Polymeric Solid-State Lithium Metal Batteries

   https://doi.org/10.1016/j.chempr.2021.06.019  

   Deng, Tao; Cao, Longsheng; He, Xinzi; Li, Ai-Min; Li, Dan; Xu, Jijian; Liu, Sufu; Bai, Panxing; Jin, Ting; Ma, Lin; et al (January 2021, Chem)

   null (Ed.)

   Composite polymer electrolytes (CPEs) for solid-state Li metal batteries (SSLBs) still suffer from gradually increased interface resistance and unconstrained Li dendrite growth. Herein, we addressed the challenges by designing a LiF-rich inorganic solid-electrolyte interphase (SEI) through introducing a fluoride-salt concentrated interlayer on CPE film. The rigid and flexible CPE helps accommodate the volume change of electrodes, while the polymeric high-concentrated electrolyte (PHCE) surface-layer regulates Li-ion flux due to the formation of a stable LiF-rich SEI via anion reduction. The designed CPE-PHCE presents enhanced ionic conductivity and high oxidation stability of > 5.0V (vs. Li/Li+). What’s more, it dramatically reduces the interfacial resistance and achieves a high critical current density of 4.5 mA cm-2 for dendrite-free cycling. The SSLBs, fabricated with thin CPE-PHCE membrane (< 100 μm) and Co-free LiNiO2 cathode, exhibit exceptional electrochemical performance and long cycling stability. This approach of SEI design can also be applied to other types of batteries. 

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2. Solid-state rigid-rod polymer composite electrolytes with nanocrystalline lithium ion pathways

   https://doi.org/10.1038/s41563-021-00995-4  

   Wang, Ying; Zanelotti, Curt J.; Wang, Xiaoen; Kerr, Robert; Jin, Liyu; Kan, Wang Hay; Dingemans, Theo J.; Forsyth, Maria; Madsen, Louis A. (May 2021, Nature Materials)

   Dusastre, Vincent (Ed.)

   A critical challenge for next-generation lithium-based batteries lies in development of electrolytes that enable thermal safety along with use of high-energy-density electrodes. We describe molecular ionic composite (MIC) electrolytes based on an aligned liquid crystalline polymer combined with ionic liquids and concentrated Li salt. This high strength (200 MPa) and non-flammable solid electrolyte possesses outstanding Li+ conductivity (1 mS·cm-1 at 25 °C) and electrochemical stability (5.6 V vs Li|Li+) while suppressing dendrite growth and exhibiting low interfacial resistance (32 Ω·cm2) and overpotentials (≤ 120 mV @ 1 mA·cm-2) during Li symmetric cell cycling. A heterogeneous salt doping process modifies a locally ordered polymer-ion assembly to incorporate an inter-grain network filled with defective LiFSI & LiBF4 nanocrystals, strongly enhancing Li+ conduction. This modular material fabrication platform shows promise for safe and high-energy-density energy storage and conversion applications, incorporating the fast transport of ceramic-like conductors with the superior flexibility of polymer electrolytes. 

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3. Organic–inorganic hybrid electrolytes from ionic liquid-functionalized octasilsesquioxane for lithium metal batteries

   https://doi.org/10.1039/C7TA04599A  

   Yang, Guang; Chanthad, Chalathorn; Oh, Hyukkeun; Ayhan, Ismail Alperen; Wang, Qing (January 2017, Journal of Materials Chemistry A)

   The use of highly conductive solid-state electrolytes to replace conventional liquid organic electrolytes enables radical improvements in the reliability, safety and performance of lithium batteries. Here, we report the synthesis and characterization of a new class of nonflammable solid electrolytes based on the grafting of ionic liquids onto octa-silsesquioxane. The electrolyte exhibits outstanding room-temperature ionic conductivity (∼4.8 × 10 −4 S cm −1 ), excellent electrochemical stability (up to 5 V relative to Li + /Li) and high thermal stability. All-solid-state Li metal batteries using the prepared electrolyte membrane are successfully cycled with high coulombic efficiencies at ambient temperature. The good cycling stability of the electrolyte against lithium has been demonstrated. This work provides a new platform for the development of solid polymer electrolytes for application in room-temperature lithium batteries. 

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4. Regulating Li‐Ion Transport through Ultrathin Molecular Membrane to Enable High‐Performance All‐Solid‐State–Battery

   https://doi.org/10.1002/smll.202303625  

   Rajendran, Sathish; George, Antony; Tang, Zian; Neumann, Christof; Turchanin, Andrey; Arava, Leela_Mohana_Reddy (June 2023, Small)

   Abstract Solid‐state lithium metal batteries with garnet‐type electrolyte provide several advantages over conventional lithium‐ion batteries, especially for safety and energy density. However, a few grand challenges such as the propagation of Li dendrites, poor interfacial contact between the solid electrolyte and the electrodes, and formation of lithium carbonate during ambient exposure over the solid‐state electrolyte prevent the viability of such batteries. Herein, an ultrathin sub‐nanometer porous carbon nanomembrane (CNM) is employed on the surface of solid‐state electrolyte (SSE) that increases the adhesion of SSE with electrodes, prevents lithium carbonate formation over the surface, regulates the flow of Li‐ions, and blocks any electronic leakage. The sub‐nanometer scale pores in CNM allow rapid permeation of Li‐ions across the electrode–electrolyte interface without the presence of any liquid medium. Additionally, CNM suppresses the propagation of Li dendrites by over sevenfold up to a current density of 0.7 mA cm⁻²and enables the cycling of all‐solid‐state batteries at low stack pressure of 2 MPa using LiFePO₄cathode and Li metal anode. The CNM provides chemical stability to the solid electrolyte for over 4 weeks of ambient exposure with less than a 4% increase in surface impurities. 

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5. NASICON Li _1.2 Mg _0.1 Zr _1.9 (PO ₄ ) ₃ Solid Electrolyte for an All‐Solid‐State Li‐Metal Battery

   https://doi.org/10.1002/smtd.202000764  

   Zhou, Qiongyu; Xu, Biyi; Chien, Po‐Hsiu; Li, Yutao; Huang, Bing; Wu, Nan; Xu, Henghui; Grundish, Nicholas S.; Hu, Yan‐Yan; Goodenough, John B. (September 2020, Small Methods)

   Abstract A thin solid electrolyte with a high Li⁺conductivity is used to separate the metallic lithium anode and the cathode in an all‐solid‐state Li‐metal battery. However, most solid Li‐ion electrolytes have a small electrochemical stability window, large interfacial resistance, and cannot block lithium‐dendrite growth when lithium is plated on charging of the cell. Mg²⁺stabilizes a rhombohedral NASICON‐structured solid electrolyte of the formula Li_1.2Mg_0.1Zr_1.9(PO₄)₃(LMZP). This solid electrolyte has Li‐ion conductivity two orders of magnitude higher at 25 °C than that of the triclinic LiZr₂(PO₄)₃.⁷Li and⁶Li NMR confirm the Li‐ions in two different crystallographic sites of the NASICON framework with 85% of the Li‐ions having a relatively higher mobility than the other 15%. The anode–electrolyte interface is further investigated with symmetric Li/LMZP/Li cell testing, while the cathode–electrolyte interface is explored with an all‐solid‐state Li/LMZP/LiFePO₄cell. The enhanced performance of these cells enabled by the Li_1.2Mg_0.1Zr_1.9(PO₄)₃solid electrolyte is stable upon repeated charge/discharge cycling. 

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